Natural ageing responses of duplex structured Mg-6%Li and Mg-6%Li-6%Zn-1.2%Y alloys have been investigated. Microstructural analyses revealed that the precipitation and coarsening process of α-Mg particles could occur in β-Li phases of both two alloys during ageing process. Since a certain amount of Mg atoms in β-Li phases were consumed for the precipitation of abundant tiny MgLiZn particles, the size of α-Mg precipitates in Mg-6%Li-6%Zn-1.2%Y alloy was relatively smaller than that in Mg-6%Li alloy. Micro hardness measurements demonstrated that with the ageing time increasing, the α-Mg phases in Mg-6%Li alloy could have a constant hardness value of 41 HV, but the contained β-Li phases exhibited a slight age-softening response. Compared with the Mg-6%Li alloy, the age-softening response of β-Li phases in Mg-6%Li-6%Zn-1.2%Y alloy was much more profound. Meanwhile, a normal age-hardening response of α-Mg phases was maintained. Tensile results indicated that obvious ageing-softening phenomenon in terms of macro tensile strength occurred in both two alloys. Failure analysis demonstrated that for the Mg-6%Li alloy, cracks were preferentially initiated at α-Mg/β-Li interfaces. For the Mg-6%Li-6%Zn-1.2%Y alloy, cracks occurred at both α-Mg/β-Li interfaces and slip bands in α-Mg and β-Li phases.